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Probing Polariton Dynamics in Trapped Ions with Phase-Coherent Two-Dimensional Spectroscopy

We devise a phase-coherent three-pulse protocol to probe the polariton dynamics in a trapped-ion quantum simulation. In contrast to conventional nonlinear signals, the presented scheme does not change the number of excitations in the system, allowing for the investigation of the dynamics within an $N$-excitation manifold. In the particular case of a filling factor one ($N$ excitations in an $N$-ion chain), the proposed interaction induces coherent transitions between a delocalized phonon superfluid and a localized atomic insulator phase. Numerical simulations of a two-ion chain demonstrate that the resulting two-dimensional spectra allow for the unambiguous identification of the distinct phases, and the two-dimensional lineshapes efficiently characterize the relevant decoherence mechanism.